A localization transition underlies the mode-coupling crossover of glasses

Coslovich, Daniele; Ninarello, Andrea; Berthier, Ludovic

doi:10.21468/scipostphys.7.6.077

Cited by 43 publications

(73 citation statements)

References 64 publications

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“…In particular, as anticipated in Ref. [23], we observe that the full disorder-averaged distribution becomes bimodal at high volume fractions, showing that we have indeed entered a deeply glassy regime that remains currently inaccessible for a standard binary Lennard-Jones liquid (see also [70]).…”

Section: Definition Of Cavity Core Overlap and Point-to-set Correlationssupporting

confidence: 84%

Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling

Berthier

Charbonneau

Coslovich

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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141

179

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Liquids relax extremely slowly on approaching the glass state. One explanation is that an entropy crisis, because of the rarefaction of available states, makes it increasingly arduous to reach equilibrium in that regime. Validating this scenario is challenging, because experiments offer limited resolution, while numerical studies lag more than eight orders of magnitude behind experimentally relevant timescales. In this work, we not only close the colossal gap between experiments and simulations but manage to create in silico configurations that have no experimental analog yet. Deploying a range of computational tools, we obtain four estimates of their configurational entropy. These measurements consistently confirm that the steep entropy decrease observed in experiments is also found in simulations, even beyond the experimental glass transition. Our numerical results thus extend the observational window into the physics of glasses and reinforce the relevance of an entropy crisis for understanding their formation.

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Section: Definition Of Cavity Core Overlap and Point-to-set Correlationssupporting

confidence: 84%

Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling

Berthier

Charbonneau

Coslovich

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

Self Cite

141

179

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“…This is not the case e.g. in [31], where swaps are used to generate dense equilibrated liquids, that are then quenched without swap toward jamming. We also expect isostaticity to be restored in algorithms for which the set of particle radii is strictly fixed, but only below some pressure p N that vanishes as N → ∞, above which our predictions should apply.…”

Section: A Jamming Transition For Soft Spheres Under Swapmentioning

confidence: 99%

Theory for Swap Acceleration near the Glass and Jamming Transitions for Continuously Polydisperse Particles

2018

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Swap algorithms can shift the glass transition to lower temperatures, a recent unexplained observation constraining the nature of this phenomenon. Here we show that swap dynamic is governed by an effective potential describing both particle interactions as well as their ability to change size. Requiring its stability is more demanding than for the potential energy alone. This result implies that stable configurations appear at lower energies with swap dynamics, and thus at lower temperatures when the liquid is cooled. The magnitude of this effect is proportional to the width of the radii distribution, and decreases with compression for finite-range purely repulsive interaction potentials. We test these predictions numerically and discuss the implications of these findings for the glass transition.We extend these results to the case of hard spheres where swap is argued to destroy meta-stable states of the free energy coarse-grained on vibrational time scales. Our analysis unravels the soft elastic modes responsible for the speed up swap induces, and allows us to predict the structure and the vibrational properties of glass configurations reachable with swap. In particular for continuously poly-disperse systems we predict the jamming transition to be dramatically altered, as we confirm numerically. A surprising practical outcome of our analysis is new algorithm that generates ultra-stable glasses by simple descent in an appropriate effective potential.

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“…In particular, it is clear that thermally activated processes in finite dimensional liquids involve only localized portions of the system, whereas the unstable modes of saddles in mean-field models are spatially delocalized. A recent numerical study [26], based on an efficient swap Monte Carlo algorithm [27,28], has tackled these two issues at once, establishing that the stationary points of several three-dimensional model liquids indeed show a sharp change around T MCT : the fraction of delocalized unstable modes vanishes at the MCT crossover temperature. At any temperature, however, saddles also possess a finite fraction of localized unstable modes, which only involve a finite number of particles, as originally envisaged by Goldstein.…”

Section: Introductionmentioning

confidence: 99%

“…At any temperature, however, saddles also possess a finite fraction of localized unstable modes, which only involve a finite number of particles, as originally envisaged by Goldstein. The extent to which the MCT transition is avoided in actual supercooled liquids thus depends on the concentration of such localized excitations [26].…”

Section: Introductionmentioning

confidence: 99%

“…In fact, the simple finite size scaling analysis of Ref. [26] was only based on the bulk average mode participation and further investigation is needed to characterize the modes' structure. Moreover, since the saddle modes progressively stabilize at low temperature, it is natural to inquire the connection between them and the stable modes populating the lowfrequency portion of the vibrational spectrum.…”

Section: Introductionmentioning

confidence: 99%

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Spatial structure of unstable normal modes in a glass-forming liquid

et al. 2021

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The phenomenology of glass-forming liquids is often described in terms of their underlying, high-dimensional potential energy surface. In particular, the statistics of stationary points sampled as a function of temperature provides useful insight into the thermodynamics and dynamics of the system. To make contact with the real space physics, however, analysis of the spatial structure of the normal modes is required. In this work, we numerically study the potential energy surface of a glass-forming ternary mixture. Starting from liquid configurations equilibrated over a broad range of temperatures using a swap Monte Carlo method, we locate the nearby stationary points and investigate the spatial architecture and the energetics of the associated unstable modes. Through this spatially-resolved analysis, originally developed to study local minima, we corroborate recent evidence that the nature of the unstable modes changes from delocalized to localized around the mode-coupling temperature. We find that the displacement amplitudes of the delocalized modes have a slowly decaying far field, whereas the localized modes consist of a core with large displacements and a rapidly decaying far field. The fractal dimension of unstable modes around the mobility edge is equal to 1, consistent with the scaling of the participation ratio. Finally, we find that around and below the mode-coupling temperature the unstable modes are localized around structural defects, characterized by a disordered local structure markedly different from the liquid's locally favored structure. These defects are similar to those associated to quasi-localized vibrations in local minima and are good candidates to predict the emergence of localized excitations at low temperature.

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A localization transition underlies the mode-coupling crossover of glasses

Cited by 43 publications

References 64 publications

Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling

Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling

Theory for Swap Acceleration near the Glass and Jamming Transitions for Continuously Polydisperse Particles

Spatial structure of unstable normal modes in a glass-forming liquid

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